Abstract
Semiconductor quantum dots have long been considered artificial atoms, but despite the overarching analogies in the strong energy-level quantization and the single-photon emission capability, their emission spectrum is far broader than typical atomic emission lines. Here, by using ab-initio molecular dynamics for simulating exciton-surface-phonon interactions in structurally dynamic CsPbBr3 quantum dots, followed by single quantum dot optical spectroscopy, we demonstrate that emission line-broadening in these quantum dots is primarily governed by the coupling of excitons to low-energy surface phonons. Mild adjustments of the surface chemical composition allow for attaining much smaller emission linewidths of 35−65 meV (vs. initial values of 70–120 meV), which are on par with the best values known for structurally rigid, colloidal II-VI quantum dots (20−60 meV). Ultra-narrow emission at room-temperature is desired for conventional light-emitting devices and paramount for emerging quantum light sources.
Original language | English |
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Article number | 2587 |
Pages (from-to) | 1-8 |
Number of pages | 8 |
Journal | Nature Communications |
Volume | 13 |
DOIs | |
Publication status | Published - 2022 |
Bibliographical note
Funding Information:G.R. acknowledges B. Benin and Dr. M. Bodnarchuk for useful discussions. M.V.K. acknowledges financial support from the Swiss Innovation Agency (Innosuisse, grant 32908.1 IP-EE) and, in part, from the European Union through Horizon 2020 research and innovation program (grant agreement No. [819740], project SCALE-HALO). I.I. acknowledges The Netherlands Organization of Scientific Research (NWO) for financial support through the Innovational Research Incentive (Vidi) Scheme (Grant No. 723.013.002) and S.C.B. acknowledges NWO for financial support through the Innovational Research Incentives (Veni) Scheme (Grant No. 722.017.011). N.Y. and V.W. acknowledge the Swiss National Supercomputing Centre (CSCS; project ID s1003). Funding for N.Y. was provided by the Swiss National Science Foundation through the Quantum Sciences and Technology NCCR. The project was also partially supported by the Air Force Office of Scientific Research and the Office of Naval Research under award number FA8655-21-1-7013, by the by the European Union’s Horizon 2020 program, through a FET Open research and innovation action under the grant agreement Grant No. 899141 (PoLLoC) and by the Swiss National Science Foundation (Grant No. 188404, “Novel inorganic light emitters: synthesis, spectroscopy and applications”).
Funding Information:
G.R. acknowledges B. Benin and Dr. M. Bodnarchuk for useful discussions. M.V.K. acknowledges financial support from the Swiss Innovation Agency (Innosuisse, grant 32908.1 IP-EE) and, in part, from the European Union through Horizon 2020 research and innovation program (grant agreement No. [819740], project SCALE-HALO). I.I. acknowledges The Netherlands Organization of Scientific Research (NWO) for financial support through the Innovational Research Incentive (Vidi) Scheme (Grant No. 723.013.002) and S.C.B. acknowledges NWO for financial support through the Innovational Research Incentives (Veni) Scheme (Grant No. 722.017.011). N.Y. and V.W. acknowledge the Swiss National Supercomputing Centre (CSCS; project ID s1003). Funding for N.Y. was provided by the Swiss National Science Foundation through the Quantum Sciences and Technology NCCR. The project was also partially supported by the Air Force Office of Scientific Research and the Office of Naval Research under award number FA8655-21-1-7013, by the by the European Union’s Horizon 2020 program, through a FET Open research and innovation action under the grant agreement Grant No. 899141 (PoLLoC) and by the Swiss National Science Foundation (Grant No. 188404, “Novel inorganic light emitters: synthesis, spectroscopy and applications”).
Publisher Copyright:
© 2022, The Author(s).
Funding
G.R. acknowledges B. Benin and Dr. M. Bodnarchuk for useful discussions. M.V.K. acknowledges financial support from the Swiss Innovation Agency (Innosuisse, grant 32908.1 IP-EE) and, in part, from the European Union through Horizon 2020 research and innovation program (grant agreement No. [819740], project SCALE-HALO). I.I. acknowledges The Netherlands Organization of Scientific Research (NWO) for financial support through the Innovational Research Incentive (Vidi) Scheme (Grant No. 723.013.002) and S.C.B. acknowledges NWO for financial support through the Innovational Research Incentives (Veni) Scheme (Grant No. 722.017.011). N.Y. and V.W. acknowledge the Swiss National Supercomputing Centre (CSCS; project ID s1003). Funding for N.Y. was provided by the Swiss National Science Foundation through the Quantum Sciences and Technology NCCR. The project was also partially supported by the Air Force Office of Scientific Research and the Office of Naval Research under award number FA8655-21-1-7013, by the by the European Union’s Horizon 2020 program, through a FET Open research and innovation action under the grant agreement Grant No. 899141 (PoLLoC) and by the Swiss National Science Foundation (Grant No. 188404, “Novel inorganic light emitters: synthesis, spectroscopy and applications”). G.R. acknowledges B. Benin and Dr. M. Bodnarchuk for useful discussions. M.V.K. acknowledges financial support from the Swiss Innovation Agency (Innosuisse, grant 32908.1 IP-EE) and, in part, from the European Union through Horizon 2020 research and innovation program (grant agreement No. [819740], project SCALE-HALO). I.I. acknowledges The Netherlands Organization of Scientific Research (NWO) for financial support through the Innovational Research Incentive (Vidi) Scheme (Grant No. 723.013.002) and S.C.B. acknowledges NWO for financial support through the Innovational Research Incentives (Veni) Scheme (Grant No. 722.017.011). N.Y. and V.W. acknowledge the Swiss National Supercomputing Centre (CSCS; project ID s1003). Funding for N.Y. was provided by the Swiss National Science Foundation through the Quantum Sciences and Technology NCCR. The project was also partially supported by the Air Force Office of Scientific Research and the Office of Naval Research under award number FA8655-21-1-7013, by the by the European Union’s Horizon 2020 program, through a FET Open research and innovation action under the grant agreement Grant No. 899141 (PoLLoC) and by the Swiss National Science Foundation (Grant No. 188404, “Novel inorganic light emitters: synthesis, spectroscopy and applications”).
Funders | Funder number |
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FET Open research and innovation action | 188404 |
Innovational Research Incentives | 722.017.011 |
Office of Naval Research | FA8655-21-1-7013 |
Air Force Office of Scientific Research | |
Horizon 2020 Framework Programme | 899141 |
European Commission | |
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung | |
Nederlandse Organisatie voor Wetenschappelijk Onderzoek | 723.013.002 |
Horizon 2020 | 819740 |
National Center of Competence in Research Quantum Science and Technology | |
Innosuisse - Schweizerische Agentur für Innovationsförderung | 32908.1 IP-EE |
Centro Svizzero di Calcolo Scientifico | s1003 |